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DOE OSTI2022

Next Generation System Analysis Model: Recently Added Features and Future Plans

To better enable informed decision-making regarding the back-end of the nuclear fuel cycle, the Integrated Waste Management System (IWMS) program within the U.S. Department of Energy, Office of Nuclear Energy (DOE-NE) has been sponsoring the development and application of system analysis tools capable of analyzing various system options for the management of spent nuclear fuel (SNF) and high-level radioactive waste (HLW).With these tools, IWMS architecture analyses are being conducted to support the future deployment of a comprehensive nuclear waste management system that considers all major back-end aspects of the nuclear fuel cycle (i.e., transportation, storage, and disposal). The Next Generation System Analysis Model (NGSAM) is an agent-based simulation software tool expressly designed to be capable of modeling features within various IWMS architectures. NGSAM imports data from Oak Ridge National Laboratory (ORNL)’s unified database (e.g., historic assembly information, thermal profiles for assembly heat, and at-reactor dry storage loadings) to ensure that each simulation initializes with a realistic representation of the state of commercial SNF in the U.S. Recent major enhancements implemented into NGSAM in the period since NGSAM was last presented at the WM2019 conference include: • Tracking of railroad escort car acquisition and buffer car acquisition • The addition of heavy haul truck (HHT) and barge routes for some sites, as well as support for user-defined inter-modal routes • Updates to the logic that checks the transportation cask thermal limit maps prior to package transport • An allocation method that predicts when reactor sites would pack assemblies from their spent fuel pools for dry storage, and prioritizes shipments directly from the pools of those reactor sites in the preceding periods (before the predicted loadings to dry storage), thus reducing the number of casks loaded into dry storage at reactor sites • The addition of “reactor site family” operational limits to restrict the number of loads of SNF taken from the pool and from dry storage at a given reactor site each year • Added support for multiple canister loading map options and packages with multiple compatible transportation overpacks • Updates to the handling of non-commercial SNF, including a new database that contains data to support the updates • Updates to allow analysis of hypothetical scenarios which include repackaging at reactor sites, e.g., for possible comparative analysis with other scenarios • Implementation of additional output reports, or modification of existing ones • The ability to generate and implement user edits via the NGSAM website • The ability to model loading SNF from pool storage at an interim storage facility (ISF) into dry storage at the ISF • The ability to model consolidating SNF from different existing storage containers at a DOE site into the same DOE standard canister • The ability to model transferring SNF casks from one transportation mode to another, e.g., from HHT to rail, referred to as transloading. These new features have improved NGSAM capabilities and users’ experience with the model. Preliminary NGSAM requirements for modeling advanced reactor fuels, reprocessing, treatment, and conditioning were considered, and this paper describes them at a high level. Other nuclear fuel cycle system analysis tools developed under sponsorship of DOE-NE, like the VISION code developed at Idaho National Laboratory, might be better suited for initial high-level analysis of those technologies and advanced fuel cycles. As technologies are developed and system concepts evolve, NGSAM could provide value by providing more detailed modeling of transport, storage, and disposal of spent fuel and wastes from advanced reactors and advanced fuel cycles at the fuel element and waste container level.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

A Brief User's Guide to the Excel ® -Based DF Calculator

To understand the importance of capturing penetrating forms of iodine as well as the other volatile radionuclides, a calculation tool was developed in the form of an Excel ® spreadsheet to estimate the overall plant decontamination factor (DF). The tool requires the user to estimate splits of the volatile radionuclides within the major portions of the reprocessing plant, speciation of iodine and individual DFs for each off-gas stream within the Used Nuclear Fuel reprocessing plant. The Impact to the overall plant DF for each volatile radionuclide is then calculated by the tool based on the specific user choices. The Excel ® spreadsheet tracks both elemental and penetrating forms of iodine separately and allows changes in the speciation of iodine at each processing step. It also tracks 3 H, 14 C and 85 Kr. This document provides a basic user's guide to the manipulation of this tool.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Remediation of the FGMSP at Sellafield: The First Transfer of Bulk Sludge - 17133

The very first bulk transfers of radioactive sludge have commenced from one of the most hazardous nuclear plants in Europe, using equipment and systems researched, designed, installed and commissioned by Jacobs as part of the ACKtiv alliance. Sellafield is a nuclear fuel reprocessing and decommissioning site, close to the village of Seascale on the coast of the Irish Sea in Cumbria, England. Sellafield incorporates the original nuclear reactor site at Windscale, which is currently undergoing decommissioning, and dismantling, and Calder Hall, the world's first nuclear power generating reactor. The first nuclear facilities were built in the 1940's.The First Generation Magnox Storage Pond (FGMSP) dates back to the 1950's as part of the UK's expanding nuclear programme and was constructed to store, cool and prepare used Magnox nuclear fuel for recycling into new fuel. It urgently needs to be emptied of 1500 cubic metres of radioactive sludge. In this paper we describe the work undertaken by Jacobs to deliver a very challenging programme of work to provide the capability to remove sludge from the pond. The FGMSP Retrievals Project was awarded in March 2007 to supply equipment and services for the removal of sludge and miscellaneous waste from the First Generation Magnox Storage Pond at Sellafield. The Project is being executed by ACKtiv Nuclear (Jacobs, Carillion and Atkins) of which Jacobs is a 40% stakeholder. ACKtiv Nuclear is a mature Joint Venture and has been operating continuously and successfully since 2002, the oldest JV still in operation on Sellafield Site. The roots of the JV can be traced back to the 1980's. The Project covers all project phases from front-end engineering through detailed design, procurement, installation and commissioning support. The Project places huge emphasis on off-Site testing and has several facilities for both installation and integrated testing. This proves equipment prior to installation in a radioactive environment. The Project has achieved success and recognition including winning the 2014 and 2015 Sellafield Business Excellence awards, as well as numerous internal Jacobs awards. The Project achieved a major decommissioning milestone in March 2016. Since the installation of a 31 m pipe-bridge in 2012, using a 1200 te mobile crane surrounded by several other facilities with nuclear inventory, the Project has successfully installed the sludge retrieval and effluent system into the FGMSP. This 4 year programme of work included 2 booster pump platforms, sludge recovery tooling, hoses, umbilicals and a deluge skip wash box which were all trialled and proven off-Site prior to installation in the pond. This milestone to commence transfer of sludge to modern stainless steel containment is a major step forward in the hazard reduction of the facility.The presentation will cover the installation of the pond de-sludging equipment, the innovations deployed that ensured that the milestone was achieved under budget and ahead of schedule, as well the benefits to the facility, the Site and the nuclear industry. It will also examine the challenges that needed to be overcome such as high dose, contamination, limited working times and space constraints. The presentation will describe why the work is of national Importance and conclude with the achievement of commencement of bulk sludge transfer to a modern facility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Human Factors and Nuclear Criticality Safety Accidents [Slides]

The agenda for the presentation is as follows: Human Factors; Accident Review (Tokai Mura, Siberian Chemical Combine); Procedures; Accident Review (Los Alamos Waste Recovery); Environmental Distractions; Accident Review (Idaho Fuel Reprocessing); and, Equipment Reliability.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Co-adsorption of I{sub 2} and H{sub 2}O on Ag{sup 0}Z and Kinetics of Iodine Silver Reaction

Co-adsorption of iodine and water by reduced silver-exchanged mordenite (Ag{sup 0}Z) is studied to support the development of multi-component adsorption models for the separation and recovery of radio isotopic gases in off-gas streams in nuclear fuel reprocessing. Single-component adsorption equilibrium data of iodine and water were obtained to determine the saturation capacity and evaluate the parameters of the generalized statistical thermodynamic adsorption (GSTA) model being developed for modeling of co-adsorption. Co-adsorption data acquisition is in progress for model validation. Kinetic data were obtained to determine the intra-particle mass transfer and reaction parameters for the adsorption models. In addition, work is in progress to obtain data of the iodine-silver reaction at various conditions to study the reaction kinetics, which will provide insight to the chemisorption process of iodine on Ag{sup 0}Z. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Removal of Tritium from the Gaseous Effluents Produced by the Recovery of Zirconium from Used Fuel Cladding

U.S. regulations will require the removal of tritium ({sup 3}H) from gaseous effluents associated with nuclear fuel reprocessing and recycling. One process that may generate {sup 3}H-containing gaseous effluents is the recovery of zirconium from used fuel cladding. A chlorination process developed by Collins et al. is designed to convert the zirconium present in Zircaloy{sup R} cladding to recoverable ZrCl{sub 4}. The greatest economic benefit from including zirconium recycle as part of a larger used nuclear fuel (UNF) recycle effort would be a decrease in the disposal cost of used fuel cladding. Used fuel cladding is considered high-level waste (HLW). As zirconium is the second largest element by mass (25%) contained in most UNF assemblies (with uranium being the largest), recovery of the zirconium could result in a substantial decrease in the amount of HLW intended for geologic disposition. The reclaimed ZrCl{sub 4} product, if sufficiently free from radioactive impurities, could then be disposed of as low-level waste or reused in nuclear applications. The chlorination process uses chlorine gas (Cl{sub 2}) and an inert carrier such as argon (Ar) to convert the zirconium present in cladding to ZrCl{sub 4}. ZrCl{sub 4} is more volatile than other components in the cladding, causing evaporation of a relatively pure gaseous ZrCl{sub 4} stream. The product ZrCl{sub 4} is recovered as a solid salt by condensation when cooled to less than about 300 deg. C. A fraction of the {sup 3}H (0-96%) produced in nuclear fuel during irradiation is found in zirconium-based cladding, possibly as zirconium hydride (the wide range is a remnant of various researchers' analyses of cladding of various irradiations and cooling times). Heating the cladding to high temperatures, such as would be done during the chlorination process, will release the {sup 3}H. At the temperatures of the zirconium recycle process, the {sup 3}H is likely to react with excess Cl{sub 2} to produce tritiated HCl ({sup 3}HCl), although this could be avoided if the cladding and fuel were treated to remove {sup 3}H prior to chlorination. A previous analysis showed that the concentration of {sup 3}HCl in the off-gas of the zirconium recycle process will be in the range of parts per billion to a few parts per million. Should {sup 3}H mitigation be required for the zirconium recycle process, it will be completed through the abatement of {sup 3}HCl from this off-gas stream. The intent of the testing described in this summary was to conduct proof-of-principle demonstrations for two {sup 3}HCl removal methods. The zirconium recycle off-gas stream differs from many industrial HCl-containing streams in that the concentration of HCl requiring removal is extremely low. Demonstrations of HCl removal at ppm concentrations were not found in the literature, making the proof-of-principle approach attractive as a way to identify the most promising method for continued development. An important consideration throughout these experiments was that current research efforts on the zirconium recycle process are conducted in a hot cell and any {sup 3}HCl removal methods should be easily deployed in a hot-cell environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

Energy Return on Investment – Fuel Recycle

This report provides a methodology and requisite data to assess the potential Energy Return On Investment (EROI) for nuclear fuel cycle alternatives, and applies that methodology to a limited set of used fuel recycle scenarios. This paper is based on a study by Lawrence Livermore National Laboratory and a parallel evaluation by AREVA Federal Services LLC, both of which were sponsored by the DOE Fuel Cycle Technologies (FCT) Program. The focus of the LLNL effort was to develop a methodology that can be used by the FCT program for such analysis that is consistent with the broader energy modeling community, and the focus of the AREVA effort was to bring industrial experience and operational data into the analysis. This cooperative effort successfully combined expertise from the energy modeling community with expertise from the nuclear industry. Energy Return on Investment is one of many figures of merit on which investment in a new energy facility or process may be judged. EROI is the ratio of the energy delivered by a facility divided by the energy used to construct, operate and decommission that facility. While EROI is not the only criterion used to make an investment decision, it has been shown that, in technologically advanced societies, energy supplies must exceed a minimum EROI. Furthermore, technological history shows a trend towards higher EROI energy supplies. EROI calculations have been performed for many components of energy technology: oil wells, wind turbines, photovoltaic modules, biofuels, and nuclear reactors. This report represents the first standalone EROI analysis of nuclear fuel reprocessing (or recycling) facilities.

02 PETROLEUM↗
DOE OSTI2016

Decommissioning Experience at Rokkasho; Standing Type Manipulator: A1000S for Dismantling Tasks - 16434

Decommissioning is a technical process which includes various steps and processes from the clean-up of radioactive materials to the progressive demolition of the plant. One of these steps is the cutting of subassemblies, like tanks, pipes or walls in small pieces suitable for the sorting and disposal. Different solutions are offered for this cutting work and can be grouped as following: - Chip forming - sawing, drilling, milling, turning etc. - Shearing - punching, stamping, scissoring. - Abrading - Grinding, lapping, polishing; water-jet. - Heat - flame cutting, plasma cutting, laser cutting. - Electro-Chemical - Etching, Electrical discharge machining (EDM). Each method has its limitations in accuracy, cost, and effect on the material. In 2013, Waelischmiller Engineering won a contract for two remote handling systems dedicated to the dismantling cell at Rokkasho Nuclear Fuel Reprocessing Facility in Japan. For this project, Inconel and other metals needed to be cut. One of the main cutting methods was decided to use of an angle grinder handled by a robotic arm. Because the use of the overhead systems (bridges and cranes) was difficult for this installation, it was determined, that the best alternative was a power manipulator A1000 installed on the floor with a pre-positioning system. The project proceeded to go forward with the adaptation of the standard A1000 with integration of a control system in a Cartesian coordinate frame; resulting in a heavy duty arm; A1000S with 6 degrees of freedom. The heavy duty power arm A1000S was developed and designed for mechanical cutting with an angle grinder, especially for thick and hard material for example stainless steel and Inconel. Cutting a thick material with an angle grinder requires repeatable precise linear motion, in order not to damage the disc. The angle grinder should be handled with a manipulator which can cut in all directions in a linear motion, since the objects which should be cut are usually very large and fixed in any direction For these requirements, the Cartesian control function was added to our standard power manipulator type A1000. In some cases, the decommissioning work includes repeated access routes or fixed access points that the manipulator arm has to pass repeatedly. For example a fixed point where the waste materials are collected, or repeated transport route that the arm has to go along for each step. For this requirement, the A1000S has been equipped with the 'Go To-Mode'. It is a 'teach and playback mode' which has been developed especially for remote operating manipulators. Quick direct teach, quick play function and an intuitive touch-panel layout are some of the features. With the Go To-Mode high working efficiency was achieved. After rigorous testing at Waelischmiller premises; the manipulator was delivered to JNFL in Rokkasho. It was found that the obtained functionality and precision can be applicable not only for the cutting with a disc grinder, but also the laser cutting method, which requires precise trajectory control. This paper will provide: - A project description, - Presentation of solution process, - Technical description of the A1000S, - Future Applications of the robotic Arm A1000S. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Dissolution of metal oxides and separation of uranium from lanthanides and actinides in supercritical carbon dioxide

This paper investigates the feasibility of extracting and separating uranium from lanthanides and other actinides by using supercritical fluid carbon dioxide (sc-CO{sub 2}) as a solvent modified with tri-n-butylphosphate (TBP) for the development of a counter current stripping technique, which would be a more efficient and environmentally benign technology for spent nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U, Pu, and Np) and europium were extracted in sc-CO{sub 2} modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, uranium/europium and uranium/plutonium extraction and separation in sc-CO{sub 2} modified with TBP is successful at nitric acid concentrations of less than 6 M and at nitric acid concentrations of less than 3 M with acetohydroxamic acid or oxalic acid, respectively. A scheme for recycling uranium from spent nuclear fuel by using sc-CO{sub 2} and counter current stripping columns is presented. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Ruthenium Volatilisation in Nuclear Waste Systems -Comparison of Ru(III)Cl{sub 3} and Ru(III)NO(NO{sub 3}){sub 3} - 17113

Ruthenium is a fission product possessed of two relatively long lived isotopes; {sup 103}Ru and {sup 106}Ru, both of which form part of the Highly Active (HA) waste raffinate during spent nuclear fuel reprocessing. During reprocessing, ruthenium, which may be in the form of the RuNO{sub 3}+ complex, encounters temperatures conducive to volatilisation. Due to ruthenium's high specific radioactivity it is important to understand the mechanism by which volatilisation occurs. Here we use combined cyclic voltammetry (CV) and electrochemical micro-gravimetry experiments in a study of both NO free Ru (III), in the form of a RuCl{sub 3} solution and NO complexed Ru (III), in the form of RuNO{sub 3}+ solutions. We do this in order to establish baseline behaviour of NO free Ru (III) and compare it to NO complexed Ru (III) to determine the effect of complexation on the system. We have observed discrete oxidations in both systems from solution phase Ru (III) to solid phase RuO{sub 2} and volatile RuO{sub 4}. Two key differences emerged between the two systems, the first being the mass changes associated with deposition and stripping of RuO{sub 2} are significantly smaller in the RuNO{sub 3}+ solutions than those for solutions of RuCl{sub 3}. The second difference is the difference in onset of volatile RuO{sub 4} generation, in the RuNO{sub 3}+ solution, RuO{sub 4} generation is 100 mV positive than that for the RuCl{sub 3} solution. This suggests NO complexation protects Ru (III) against oxidation and, to a certain extent, volatilisation as RuO{sub 4}. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Direct measurement of 235 U in spent fuel rods with Gamma-ray mirrors

We report here that direct measurement of plutonium and uranium X-rays and gamma-rays is a highly desirable nondestructive analysis method for the use in reprocessing fuel environments. The high background and intense radiation from spent fuel make direct measurements difficult to implement since the relatively low activity of uranium and plutonium is masked by the high activity from fission products. To overcome this problem, we make use of a grazing incidence optic to selectively reflect K α and K β fluorescence of Special Nuclear Materials (SNM) into a high-purity position-sensitive germanium detector and obtain their relative ratios.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Review of recent developments in iodine wasteform production

Radioiodine capture and immobilization is not only important to consider during the operation of reactors (i.e., I-131), during nuclear accidents (i.e., I-131 and I-129) or nuclear fuel reprocessing (i.e., I-131 and I-129), but also during disposal of nuclear wastes (i.e., I-129). Most disposal plans for I-129-containing waste forms (including spent nuclear fuel) propose to store them in underground repositories. Here, iodine can be highly mobile and, given its radiotoxicity, needs to be carefully managed to minimize long-term environmental impacts arising from disposal. Typically, any process that has been used to capture iodine from reprocessing or in a reactor is not suitable for direct disposal, rather conversion into a wasteform for disposal is required. The objectives of these materials are to use either chemical immobilization or physical encapsulation to reduce the leaching of iodine by groundwaters. Some of the more recent ideas have been to design capture materials that better align with disposal concepts, making the industrial processing requirements easier. Research on iodine capture materials and wasteforms has been extensive. This review will act as both an update on the state of the research since the last time it was comprehensively summarized, and an evaluation of the industrial techniques required to create the proposed iodine wasteforms in terms of resulting material chemistry and applicability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Determination of plutonium in spent nuclear fuel using high resolution X-ray

Characterization of Pu is an essential aspect of safeguards operations at nuclear fuel reprocessing facilities. A novel analysis technique called hiRX (high resolution X-ray) has been developed for the direct measurement of Pu in spent nuclear fuel dissolver solutions. hiRX is based on monochromatic wavelength dispersive X-ray fluorescence (MWDXRF), which provides enhanced sensitivity and specificity compared with conventional XRF techniques. A breadboard setup of the hiRX instrument was calibrated using spiked surrogate spent fuel (SSF) standards prepared as dried residues. Samples of actual spent fuel were utilized to evaluate the performance of the hiRX. The direct detection of just 39 ng of Pu is demonstrated. Initial quantitative results, with error of 4–27% and precision of 2% relative standard deviation (RSD), were obtained for spent fuel samples. The limit of detection for Pu (100 s) within an excitation spot of 200 μm diameter was 375 pg. This study demonstrates the potential for the hiRX technique to be utilized for the rapid, accurate, and precise determination of Pu. Moreover, the results highlight the analytical capability of hiRX for other applications requiring sensitive and selective nondestructive analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2011

SPECTROSCOPIC ON-LINE MONITORING FOR PROCESS CONTROL AND SAFEGUARDING OF RADIOCHEMICAL STREAMS

There is a renewed interest worldwide to promote the use of nuclear power and close the nuclear fuel cycle. The long term successful use of nuclear power is critically dependent upon adequate and safe processing and disposition of the spent nuclear fuel. Liquid-liquid extraction is a separation technique commonly employed for the processing of the dissolved spent nuclear fuel. The instrumentation used to monitor these processes must be robust, require little or no maintenance, and be able to withstand harsh environments such as high radiation fields and aggressive chemical matrices. In addition, the ability for continuous online monitoring allows for numerous benefits. Our team experimentally assessed the potential of Raman and spectrophotometric techniques for on-line real-time monitoring of the U(VI)/nitrate ion/nitric acid and Pu(IV)/Np(V)/Nd(III), respectively, in solutions relevant to spent fuel reprocessing. Both techniques demonstrated robust performance in the repetitive batch measurements of each analyte in a wide concentration range using simulant and commercial dissolved spent fuel solutions. Static spectroscopic measurements served as training sets for the multivariate data analysis to obtain partial least squares predictive models, which were validated using on-line centrifugal contactor extraction tests. This paper summarizes or methodology and results of the U(VI)/nitrate system as a specific example.

separations, PUREX, U, Pu, Np, nitic acid, TBP dod↗
DOE OSTI2014

Aging of Iodine-Loaded Silver Mordenite in NO2

Used nuclear fuel facilities need to control and minimize radioactive emissions. Off-gas systems are designed to remove radioactive contaminants, such as 85Kr, 14C, 3H, and 129I. In an off-gas system, any capture material will be exposed to a gas stream for months at a time. This gas stream may be at elevated temperature and could contain water, NOx gas, or a variety of other constituents comprising the dissolver off-gas stream in a nuclear fuel reprocessing plant. For this reason, it is important to evaluate the effects of long-term exposure, or aging, on proposed capture materials. One material under consideration is reduced silver mordenite (Ag0Z), which is recognized for its efficient iodine capture properties. Iodine is immobilized on Ag0Z as AgI, a solid with low volatility (m.p. ≥ 500°C). The aim of this study was to determine whether extended aging at elevated temperature in a nominally 2% NO2 environment would result in a loss of immobilized iodine from this material due to either physical or chemical changes that might occur during aging. Charges of iodine-loaded reduced silver mordenite (I2-Ag0Z) were exposed to a 2% NO2 environment for 1, 2, 3, and 4 months at 150°C, then analyzed for iodine losses The aging study was completed successfully. The material did not visibly change color or form. The results demonstrate that no significant iodine loss was observed over the course of 4 months of 2% NO2 aging of I2-Ag0Z at elevated temperature within the margin of error and the variability (~10%) in the loading along the beds. This provides assurance that iodine will remain immobilized on Ag0Z during extended online use in an off-gas capture treatment system. Future tests should expose I2-Ag0Z to progressively more complex feed gases in an effort to accurately replicate the conditions expected in a reprocessing facility.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

Fuel Age Impacts on Gaseous Fission Product Capture During Separations

As a result of fuel reprocessing, volatile radionuclides will be released from the facility stack if no processes are put in place to remove them. The radionuclides that are of concern in this document are 3 H, 14 C, 85 Kr, and 129 I. The question we attempt to answer is how efficient must this removal process be for each of these radionuclides? To answer this question, we examine the three regulations that may impact the degree to which these radionuclides must be reduced before process gases can be released from the facility. These regulations are 40 CFR 61 (EPA 2010a), 40 CFR 190(EPA 2010b), and 10 CFR 20 (NRC 2012), and they apply to the total radonuclide release and to the dose to a particular organ – the thyroid. Because these doses can be divided amongst all the radionuclides in different ways and even within the four radionuclides in question, several cases are studied. These cases consider for the four analyzed radionuclides inventories produced for three fuel types—pressurized water reactor uranium oxide (PWR UOX), pressurized water reactor mixed oxide (PWR MOX), and advanced high-temperature gas-cooled reactor (AHTGR)—several burnup values and time out of reactor extending to 200 y. Doses to the maximum exposed individual (MEI) are calculated with the EPA code CAP-88 (Rosnick 2007, 1992). Two dose cases are considered. The first case, perhaps unrealistic, assumes that all of the allowable dose is assigned to the volatile radionuclides. In lieu of this, for the second case a value of 10% of the allowable dose is arbitrarily selected to be assigned to the volatile radionuclides. The required decontamination factors (DFs) are calculated for both of these cases, including the case for the thyroid dose for which 14 C and 129 I are the main contributors. However, for completeness, for one fuel type and burnup, additional cases are provided, allowing 25% and 50% of the allowable dose to be assigned to the volatile radionuclides. Because 3 H and 85 Kr have relatively short half-lives, 12.3 y and 10.7 y, respectively, the dose decreases with the time from when the fuel is removed from the reactor to the time it is processed (herein “fuel age”). One possible strategy for limiting the discharges of these short halflife radionuclides is to allow the fuel to age to take advantage of radioactive decay. Therefore, the doses and required DFs are calculated as a function of fuel age. Here we calculate, given the above constraints and assumptions, the minimum ages for each fuel type that would not require additional effluent controls for the shorter half-life volatile radionuclides based on dose considerations. With respect to 129 I doses, we find that the highest dose is calculated with iodine as a fine particulate. The dose scales as the fraction of the total 129 I that is particulate. Therefore, we assume for all of our calculations that 100% of the 129 I is particulate and allow the user of the results given here to scale our calculated doses to their needs. To summarize the data given in the body and appendices of this report, we find that the principal isotopes of concern are 3 H and 129 I, the latter requiring the highest DFs. The maximum DF value for 129 I is 8000 for the illustrated cases. The required DF for 3 H could be as high as 720, depending on the age of the fuel processed. The DF for 85 Kr could be up to ~60, depending on fuel age. The DF for 14 C is in many cases 1 (no treatment required) but could be as high as 30. The DFs required are within the range of DFs that are reported for the capture technologies that are available for the volatile radionuclides. Achieving the required 129 I and 3 H DFs is more challenging. Variations in stack design and other design factors may also significantly impact the DF requirements.

carbon-14↗